Process for the synthetic production of nitrogen compounds.



. 2 5; E. A. STAHKE.

PROCESS FOR THE SYNWEHC FRGQUQUON 0F MT'ROGEN COMPOUNDS. APPLICATIONHLEL MAY 3. i915 1,206,155. Patented Nw zs, 1916.

PAUL A. STARKE AND ERIC A. STARKE, OF BERKELEY, CALIFORNIA, ASSIGNOBS T0STANDARD OIL COMPANY, OF RICHMOND, CALIFORNIA, A CQEPORATION OF CALI-FORNIA.

PROCESS FOR THE SYNTHETIC To all whom it may concern Be it known thatwe, PAUL A. STARKE and Euro A. STARKE, citizens of the United States,residing at Berkeley, in the county of Alameda and State of California,have invented certain new and useful Improvements in Processes for theSynthetic Production of Nitrogen Compounds, of which the following is aspecification.

Our invention relates to the synthetic pro- I duction of nitrogencompounds, such as oyanids or cyanogen compounds andammonia, and moreparticularly to a process of obtaining the same from methane. Theprocess is based upon our discovery that by using methane as the sourceof production the catalyzer may be free of carbon.

\Ve are aware of synthetic processes in which artificially preparedgases, mixed with nitrogen, are passed through a heated catalytic mass.Such gases have always been composed of hydrogen and carbon monoxid withvarying proportions of hydrocarbon gases, and it has been essential thatcarbon and other reducing agents, such as alkali metals, boron, etc., bepresent in the catalytic mass.

We have found that methane may be used as the source of production ofthe cyanid withoutthe presence of carbon or other reducing agents in thecatalytic mass, as said gas itself furnishes the necessary carbon forthe reaction. In this discovery lies the advantage of our process, inthat we are able to utilize natural gas and commercial alkalis as thesource of production, with the result of both cheapening the processandincreasing the production.

\Ve may here state that we employ the term methane generically, to coverand include all forms of natural gas, whether petroleum gases, or marshgases, or any natural gas of the paraflin series, which are, as is wellknown, simply impure forms of methane.

Our process consists, in general, in first mixing methane with nitrogen;then preparing the catalytic mass, then passing the mixture of methaneand nitrogen through the catalytic mass at suitable temperature for thedesired reactions; and then recovering from the catalyzer the nitrogencompounds. These steps, in their order, will now be more fullyexplained) Specification of Letters Patent.

PRODUCTION OF NITROGEN COMPOUNDS.

Patented Nov. 28, 1916.

Application filed May a, 1915. Serial No. 25,608.

The methane may be any natural gas of the paraflin series. The nitrogenmaybe had from any source and produced in any suitable manner. Inpractice We use atmospheric nitrogen, by simply mixing air with themethane. The proportion of'nitrogen to be used with the methane mayvary, but we find that a mixture of about equal volumes is best, asin'such proportion its activity as a reducing agent is considerablyincreased. The catalytic 'mass is best a mixture of an alkali or analkali metal salt, an alkaline earth, and a metal of the iron group. Thealkali may, for example,'be sodium or potassium oxid or carbonate, orthe salt may be potassium or sodium sulfate, or these alkalis and saltsmay be mixed. The alkaline earth may be the oxid of calcium, barium ormagnesium, or these may be mixed. The metal may be iron or aluminum,either in the metallic form or in combination,-such as sodium aluminate,sodium iron oxid, or barium aluminate or iron oxid. Vi e find that whenthe catalytic mass contains only an alkali or a mixture of alkalis orsalts of'alkali metals the amount of cyanid is small, and we furtherfind thateven when, in addition, an alkaline earth is incorporated inthe catalytic mass, the yield of cyanid though greatly increased, isstill insuflicient to warrant commercial production. Finally, we findthat when the metals comprising the iron group, that is, any salts ofiron, nickel, cobalt, chromium or aluminum are also present in thecatalyzer, the yield is so materially influenced as to place the processon a commercial basis. It makes little difi'erence in what form themetal is present, that is, whether it be in the metallic state or insome form of chemical combination.

As an alkaline salt we prefer the carbonates, such as sodium orpotassium carbonates.

Chlorids can also be employed as these transhowever, a, benefit, ,butzfor a. difierent rea son, namely, that it mayfrender the mass moreporqas and thus permitQthe-jntimate.

We claim 1. The process for the synthetic production of nitrogencompounds which consists in first making a mixture of methane andnitrogen; then passing said mixture through a heated catalytic massdevoid of carbon as a chemical reactive agent to form therein cyanogencompounds; and, finally, recovering the nitrogen compounds from saidmass.

2. The process for the synthetic production of nitrogen compounds whichconsists in first making a mixture of methane and nitrogen; then passingsaid mixture through a heated catalytic mass devoid of carbon as achemical reactive agent and composed of alkaline substances With whichis mixed a metal of the iron group, to form therein cyanogen compounds;and, finally, recovering the nitrogen compounds from said mass.

The process for the synthetic produc tion of nitrogen compounds whichconsists in first making a mixture of methane and nitrogen; then passingsaid mixture through a heated catalytic mass devoid of carbon as a chemialneactive agent and composed of a mixtui ig a metal of the iron groupto form cyanogen compounds in said mass; and, finally, recovering thenitrogen compounds fromsaid mass.

4. In the process for the synthetic pro duction of nitrogen compounds bycatalysis, that step which consists in subjecting a mixture of methaneand atmospheric air, under a temperature not lower than 600 degreescentigrade, to a catalytic agent devoid of carbon as a chemical reactiveagent.

In testimony whereof We have signed our names to this specification inthe presence of two subscribing witnesses.

PAUL A. STARKE. ERIC A. STARKE.

WVitnesses WM. F. Boo'rH, D. B. RICHARDS.

(it alkalis, alkaline earths and

